# US 12,110,598 B2 · Manufacturing method for alloy material, alloy material, electrochemical element, electrochemical module, electrochemical device, energy system and solid oxide fuel cell

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- Number: US 12,110,598 B2
- Document ID: US12110598B2
- Status: Granted
- Kind: B2
- Application number: 18/235,219
- Filed: 2023-08-17
- Published: 2023-12-07
- Granted: 2024-10-08
- Earliest claimed: 2017-03-31
- Assignees: Osaka Gas Co., Ltd.
- Applicants: Osaka Gas Co., Ltd.
- Inventors: Mitsuaki Echigo; Hisao Ohnishi
- Web page: https://patentgrep.com/patent/US12110598B2

## CPC

- C23C 8/16: using oxygen-containing compounds, e.g. water, carbon dioxide
- C23C 8/18: Oxidising of ferrous surfaces
- C22C 38/18: containing chromium
- C22C 38/50: with titanium or zirconium
- C23C 18/1689: {After-treatment}
- C23C 18/1692: {Heat-treatment}
- C23C 18/32: Coating with nickel, cobalt or mixtures thereof with phosphorus or boron (C23C18/50 takes precedence)
- C23C 28/04: only coatings of inorganic non-metallic material
- C23C 28/345: {with at least one oxide layer}
- C25D 3/12: of nickel or cobalt
- C25D 5/48: After-treatment of electroplated surfaces
- C25D 5/50: by heat-treatment
- H01M 8/0232: Metals or alloys
- H01M 8/0245: in the form of layered or coated products
- H01M 8/1226: characterised by the supporting layer
- H01M 8/2432: Grouping of unit cells of planar configuration
- H01M 8/2484: characterised by external manifolds
- C22C 38/04: containing manganese
- C22C 38/42: with copper
- C22C 38/48: with niobium or tantalum
- H01M 2008/1293: {Fuel cells with solid oxide electrolytes}
- Y02E 60/50: Fuel cells
- Y02P 20/129: Energy recovery, e.g. by cogeneration, H2recovery or pressure recovery turbines
- Y02P 70/50: Manufacturing or production processes characterised by the final manufactured product
- C23C: COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL (making metal-coated products by extrusion B21C23/22; covering with metal by connecting pre-existing layers to articles, see the relevant places, e.g. B21D39/00, B23K; metallising of glass C03C; metallising mortars, concrete, artificial stone, ceramics or natural stone C04B41/00; enamelling of, or applying a vitreous layer to, metals C23D; treating metal surfaces or coating of metals by electrolysis or electrophoresis C25D; single-crystal film growth C30B; by metallising textiles D06M11/83; decorating textiles by locally metallising D06Q1/04)
- C22C: ALLOYS (treatment of alloys C21D, C22F)
- C25D: PROCESSES FOR THE ELECTROLYTIC OR ELECTROPHORETIC PRODUCTION OF COATINGS; ELECTROFORMING; APPARATUS THEREFOR
- H01M: PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- Y02E: REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02P: CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS

## Abstract

Provided is an alloy material including a metal oxide thin layer that can be formed using a simple method at low cost and can further suppress volatilization of Cr, which causes deterioration of a fuel cell, compared with a case where conventional expensive materials are used. Disclosed is a manufacturing method for an alloy material including a coating treatment step for coating a substrate made of a Fe—Cr based alloy with Co, and an oxidation treatment step for performing oxidation treatment on the substrate in a moisture-containing atmosphere after the coating treatment step.

## Claims

### Claim 1

An electrochemical element in which at least an electrode layer, an electrolyte layer, and a counter electrode layer are provided on and/or over an alloy material comprising:
a substrate made of a Fe—Cr based alloy; and
a layer formed on and/or over the substrate,
wherein the layer contains Co, and
wherein a Co-containing region is formed at a portion inside the substrate which portion faces an interface between the substrate and the layer.

### Claim 2 (depends on 1)

An electrochemical module in which a plurality of the electrochemical elements according to claim 1 are arranged in an assembled state.

### Claim 3 (depends on 2)

An electrochemical device comprising at least the electrochemical module according to claim 2 and a reformer and comprising a fuel supply unit which supplies fuel gas containing a reducible component to the electrochemical module.

### Claim 4 (depends on 2)

An electrochemical device comprising at least the electrochemical module according to claim 2 and an inverter that extracts electrical power from the electrochemical module.

### Claim 5 (depends on 1)

The electrochemical element according to claim 1, wherein:
the layer comprises a first layer and a second layer,
the first layer is formed on and/or over the substrate and is made of a metal oxide that contains Cr, and
the second layer is formed on and/or over the first layer as a metal oxide layer that contains Co.

### Claim 6 (depends on 5)

The electrochemical element to claim 5, wherein the second layer contains Mn.

### Claim 7 (depends on 1)

The electrochemical element according to claim 1, wherein the Fe—Cr based alloy of the substrate contains Mn in an amount of 0.05 mass % or more.

### Claim 8 (depends on 1)

The electrochemical element according to claim 1, wherein the Fe—Cr based alloy of the substrate is any one of a Fe—Cr based alloy that contains Ti in an amount of 0.15 mass % or more and 1.0 mass % or less, a Fe—Cr based alloy that contains Zr in an amount of 0.15 mass % or more and 1.0 mass % or less, and a Fe—Cr based alloy that contains Ti and Zr, the total content of Ti and Zr being 0.15 mass % or more and 1.0 mass % or less.

### Claim 9 (depends on 1)

The electrochemical element according to claim 1, wherein the Fe—Cr based alloy of the substrate contains Cu in an amount of 0.10 mass % or more and 1.0 mass % or less.

### Claim 10

An electrochemical device comprising at least one of a separator, a manifold, an interconnector, and a current collector,
wherein at least one of the separator, the manifold, the interconnector, and the current collector is formed of an alloy material comprising:
a substrate made of a Fe—Cr based alloy; and
a layer formed on and/or over the substrate,
wherein the layer contains Co, and
wherein a Co-containing region is formed at a portion inside the substrate which portion faces an interface between the substrate and the layer.

### Claim 11 (depends on 1)

The electrochemical element according to claim 1, wherein the Fe—Cr based alloy of the substrate contains Cr in an amount of 18 mass % or more and 25 mass % or less.

### Claim 12 (depends on 10)

The electrochemical device according to claim 10, wherein:
the layer comprises a first layer and a second layer,
the first layer is formed on and/or over the substrate and is made of a metal oxide that contains Cr, and
the second layer is formed on and/or over the first layer as a metal oxide layer that contains Co.

### Claim 13 (depends on 12)

The electrochemical device to claim 12, wherein the second layer contains Mn.

### Claim 14 (depends on 10)

The electrochemical element according to claim 10, wherein the Fe—Cr based alloy of the substrate contains Mn in an amount of 0.05 mass % or more.

### Claim 15 (depends on 10)

The electrochemical device according to claim 10, wherein the Fe—Cr based alloy of the substrate is any one of a Fe—Cr based alloy that contains Ti in an amount of 0.15 mass % or more and 1.0 mass % or less, a Fe—Cr based alloy that contains Zr in an amount of 0.15 mass % or more and 1.0 mass % or less, and a Fe—Cr based alloy that contains Ti and Zr, the total content of Ti and Zr being 0.15 mass % or more and 1.0 mass % or less.

### Claim 16 (depends on 10)

The electrochemical device according to claim 10, wherein the Fe—Cr based alloy of the substrate contains Cu in an amount of 0.10 mass % or more and 1.0 mass % or less.

### Claim 17 (depends on 10)

The electrochemical device according to claim 10, wherein the Fe—Cr based alloy of the substrate contains Cr in an amount of 18 mass % or more and 25 mass % or less.

### Claim 18 (depends on 3)

An energy system comprising:
the electrochemical device according to claim 3; and
a waste heat management unit that reuses heat discharged from the electrochemical device.

### Claim 19 (depends on 1)

A solid oxide fuel cell comprising the electrochemical element according to claim 1, wherein a power generation reaction is caused in the electrochemical element.